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Impact of microwave-field inhomogeneity in an alkali vapour cell using Ramsey double-resonance spectroscopy

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Abstract. We numerically and experimentally evaluate the impact of the inhomogeneity of the microwave field in the cavity used to perform double-resonance (DR) Ramsey spectroscopy in a buffer gas alkali vapour cell. The Ramsey spectrum is numerically simulated using a simple theoretical model and taking into account the field distribution in a magnetron-type microwave resonator. An experi-mental evaluation is performed using a DR pulsed optically pumped (POP) atomic clock. It is shown that the sensitivity to the micro-wave power of the DR POP clock can be reproduced from the com-bination of two inhomogeneities across the vapour cell: microwave field inhomogeneity and atomic ground-state resonance frequency inhomogeneity. Finally, we present the existence of an optimum operation point for which the microwave power sensitivity of our DR POP clock is reduced by two orders of magnitude. It leads into a long-term frequency stability of 1 ´ 10–14.

Keywords: microwave-power frequency shift, microwave field ampli-tude inhomogeneity, double-resonance clock, POP clock, rubidium, magnetron-type cavity, vapour cell.

1. Introduction

Vapour-cell  frequency  standards  combine  reduced  volume  and power consumption while maintaining excellent frequency  stability performances. Among the laboratory prototype clocks  are continuous-wave (cw) [1 – 3] or pulsed optically pumped  (POP)  [4 – 6]  double-resonance  (DR)  clocks,  or  cw  [7]  or  pulsed  [8, 9]  coherent  population  trapping  (CPT)  clocks.  Compact cold caesium atomic clocks [10] are also currently  in development. Most of the recent laboratory atomic clock  prototypes demonstrate frequency stabilities at t = 1 s in the  range  of  (2 – 6) ´ 10–13 t–1/2  and  reach  in  the  medium-to-long  terms  the  level  of  10–14,  for  integration  times  larger  than  t > 104 s. The main limiting factors on these time scales arise  from  the  clock  frequency  sensitivities  to  instabilities  in  the  atoms’  environment:  light  source’s  intensity  or  frequency  through  the  light  shift  effects,  the  microwave  power,  other  environmental  parameters  such  as  residual  static  magnetic  field, temperature, atmospheric pressure [11], and humidity. 

Ultimately,  the  long-term  stability  of  the  atomic  clock  is  limited by aging processes.

In the case of rubidium (Rb) vapour-cell DR POP atomic  clocks, the origin of the clock frequency sensitivity to the vari-ations  of  the  amplitude  of  the  microwave  field  in  the  reso-nance  cell  was  identified  to  result  from  two  distinct mecha-nisms. The first mechanism is due to the cavity pulling effect  which is related to the frequency mismatch between the rubid-ium ground state splitting frequency and the microwave-cavity  resonance frequency [12]. The second mechanism is the posi-tion-shift  effect.  The  resonance  frequency  of  a  group  of  Rb  atoms  will  be  different  from  another  group  of  atoms  in  the  vapour cell because of inhomogeneous electric, magnetic and  electro-magnetic (EM) fields. The measured clock frequency is  a weighted average of the resonance frequencies of each group  of atom. Any change in the microwave power will modify the  weighting  inside  the  vapour  cell  which  results  in  a  clock  fre-quency change [13, 14]. Note that this description is valid only  for buffer gas cells in which the change of position of each atom  during a Ramsey cycle may be considered as negligible.

In  this  work,  we  evaluate  the  impact  of  the  microwave  magnetic field amplitude inhomogeneity and its weighting of  the  atomic  resonance  frequencies  distributed  within  the  cell  on the pro perties of the central Ramsey fringe with an empha-sis  on  its  (1)  contrast,  (2)  full-width-at-half-maximum  (FWHM),  and  (3)  central  fringe  centre-frequency  (CFCF)  detuning  obtained  in  a  DR  POP  Rb  clock  experiment.  We  first  review  the  basic  theoretical  model  describing  the  DR  POP  scheme  in  the  3-level  approximation.  We  decompose  our vapour cell into a 3D mesh (of 1800 points) where each  point of the mesh has different value of microwave magnetic  field amplitude (based on the simulated microwave magnetic  field  amplitude  distribution  for  the  magnetron-type  micro-wave cavity used in our Rb clock prototype) and a different  atomic  resonance  frequency.  We  evaluate  the  impact  of  the  microwave magnetic field amplitude inhomogeneity by mea-suring  the  mentioned  characteristics  of  the  Ramsey  central  fringe in our DR POP clock prototype for various microwave  powers. Finally, the results are discussed and we demonstrate  that the microwave-power sensitivity of our DR POP atomic  clock  can  be  reproduced  from  the  presence  of  microwave  magnetic field amplitude inhomogeneity and atomic ground-state resonance frequency distribution across the cell.

2. Theoretical model

In  this  section,  the  double-resonance  interaction  (Fig.  1a)  in  the  3-level  approximation  of  the 87Rb  D

2  line  (Fig.  1c)  is  described  according  to  the  theory  presented  in  [12,  15]. 

Impact of microwave-field inhomogeneity in an alkali vapour cell

using Ramsey double-resonance spectroscopy

W. Moreno, M. Pellaton, C. Affolderbach, N. Almat, M. Gharavipour, F. Gruet, G. Mileti

W. Moreno, M. Pellaton, C. Affolderbach, N. Almat, M. Gharavipour, F. Gruet, G. Mileti  Laboratoire Temps-Fréquence, Institut de 

Physique, Université de Neuchâtel, Avenue de Bellevaux 51, 2000  Neuchâtel, Switzerland; e-mail: [email protected];  [email protected]

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The  DR  POP  scheme  theory  can  be  understood  physically  using  Bloch’s  vector  representation.  The  atomic  population  is  optically  pumped  into  one  of  the  ground  state  (Fig.  1b).  As demonstrated in [12, 15], the state of the atomic popula-tion, at the end of the Ramsey scheme, can be expressed as the  matrix product (in the rotating wave approximation):

R(tend) = Mm(tm)MD(TRamsey)Mm(tm)R(0),  (1) where  tend  =  TRamsey  +2tm  is  the  duration  of  the  Ramsey  scheme and t = 0 corresponds to the end of optical pumping.  The  matrix  Mm  describes  the  microwave  interaction  and  is  given by [12, 15]: Mm(t) = ( ) ( ) ( ) ( ) ( ) ( ( )) ( ) ( ( )) ( ) cos sin sin sin cos cos sin cos cos t t b t t b t b t b t b t b t 1 1 m m m m m m 2 2 2 2 2 2 2 2 x x x x x x x x x x x x x x x x x W W W W W W - + -+ J L K K K K K K K N P O O O O O O O  .  (2) Here, x2 = W2 m + b2, where b is the microwave Rabi frequency.  In  the  case  of  zero  microwave  detuning,  the  matrix  Mm  is 

reduced to a rotation matrix around the y axis by an angle 

q  =  btm,  which  is  usually  called  the  microwave  pulse  area  and represents the rotation angle of the Bloch vector during  one microwave pulse in the Bloch sphere representation. The  matrix  MD  describes  the  free  evolution  of  the  Bloch  vector  R(t) and is given by [12, 15]: MD(t) = ( ) ( ) ( ) ( ) ( ) ( ) ( ) ( ) ( ) exp cos exp sin exp sin exp cos exp t t t t t t t t t 0 0 0 0 m m m m 2 2 2 2 1 g g g g g W W W W --

-f

p

,  (3) ( ) ( ( )) ( ( )) ( ) Re Im R t t t t 2 2 12 12 d d D =

f

p

, (4)

where  d12  is  the  ground  state  coherence;  D = r22  –  r11;  and  rii is the density of atoms in one of the ground state levels | iñ. 

The  Ramsey  spectrum  is  obtained  by  computing  R3(tend)  =  D (tend)  as  a  function  of  the  microwave  frequency  detuning  Wm . The cell volume is decomposed into a mesh with the divi-sion sizes given below.  Size of the absorption cell  diameter

/

mm   .  .  .   25       length

/

mm .  .  .   25 Size of the subdivisions  Dx

/

mm    .  .  .  2 Dy

/

mm .  .  .  2 Dz

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mm .  .  .  1 Optical absorption cross section  s13

/

m2   .  .  .  1.3 ´ 10–15 s23

/

m2   .  .  .  1.6 ´ 10–15 n0

/

m–3   .  .  .  2.89 ´ 1017 Theoretical D2 linewidth of the optical transition,  G/GHz .  .  .  2.5 Population and coherence relaxation rates  g1

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Hz .  .  .  . 360 g2

/

Hz .  .  .  . 340 A certain value of the microwave magnetic field amplitude is  associated to each point of the mesh and the Ramsey spectra  are  computed  using  the  matrix  product  (1)  at  each  point  assuming a perfect optical pumping. With the Beer – Lambert  law applied for the optical detection pulse (see Fig. 1b), the  intensity at the end of the vapour cell is given by: I j ( ) ( )exp ( ) I Li cell 0 i n ii z j 3 0 T s r = e-

/

z o, (5) where I(0) is the detection light intensity at the entrance of the  vapour  cell;  si3  is  the  optical  absorption  cross  section  for  the transition | iñ ® |3ñ; rii(zj) is the density of atoms in one of 

the ground state levels at the point zj

; and Dz is the z-axis inte-gration step. 

3. Experimental setup

The  numerical  simulations  are  compared  with  the  Ramsey  spectra measured using our POP DR Rb atomic clock proto-type. Details of the clock were previously presented in [3, 5].  Our clock prototype is based on a home-made 87Rb-enriched  vapour glass cell, 25-mm long and 25 mm in diameter, with a  D2 780.2 nm 384.2 THz G g1 g2 TRamsey Tp t Td z Vapour cell Microwave cavity Light Microwave tm Hz b a c tm D0 Wm wL wm |1ñ |2ñ |3ñ 5p2P 3/2 5s2S 1/2 87Rb F = 2 F = 1

Figure 1. (a)  Double-resonance  interaction  scheme,  (b)  POP  timing 

scheme,  and  (c)  three-level  approximation  of  the 87Rb  D

2  line.  Here,  Hz is magnetic field strength of the microwave signal; wL and wm are the 

optical and microwave frequencies; Di

0 = w3i – wL is the laser frequency 

detuning  (i  =  1,  2  are  the  numbers  of  the  components  of  the  ground  state); Wm = w21 – wm

 is the microwave frequency detuning; G  is the ex-ited state linewidth; g1 and g2

 are the ground state population and co-herence relaxation rates, respectively; Tp, tm, and Td are the duration of 

the laser optical pump, microwave, and optical detection pulses, respec-tively; and TRamsey is the Ramsey delay.

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buffer gas mixture of argon and nitrogen (PAr /PN2 = 1.6). The  laser  used  for  both  optical  pumping  and  detection  pulses  is  frequency stabilised to one of the sub-Doppler transition fre-quencies, | 2S 1/2, F = 1 ñ ® | 2P3/2, F' = 0 / F' = 1 ñ or | 2S1/2, F = 2 ñ ®  | 2P 3/2, F' = 3 ñ, of the 87Rb D2 line. The microwave cavity is  a magnetron-type cavity [16] with a loaded quality factor of  QL  = 185. The microwave magnetic field amplitude distribu-tion is shown in Fig. 2. The clock setup is operated in the POP  DR scheme [4] where the duration of each pulse is set as fol-lows: Tp = 0.4 ms, tm = 0.3 ms, TRamsey = 3 ms, and Td = 0.7 ms.

4. Results

In  this  section,  the  Ramsey  spectrum  is  obtained  in  three  cases:  numerical  simulation  with  homogeneous  microwave  magnetic  field  amplitude  distribution,  numerical  simulation  with  inhomogeneous  microwave  magnetic  field  amplitude  distribution,  and  measurement  using  our  POP  Rb  clock.  These Ramsey spectra are obtained for different values of the  microwave pulse area q = btm with b µ  Pm and for a fixed  tm. Here, Pm is the microwave power. For each spectrum, we  are  interested  in  its  contrast,  full-width-at-half-maximum,  and CFCF detuning.

4.1. Ramsey spectrum

Figure 3 presents the calculated light intensity at the end of  the  vapour  cell  I(q =  p/2)  as  a  function  of  the  microwave  frequency detuning Wm and the measured Ramsey spectrum.  The  light  intensity  is  obtained  according  to  equation  (5)  after one cycle of microwave interrogation described by equa-tion  (1)  in  the  case  of p/2  microwave  pulses  considering  the  microwave  magnetic  field  amplitude  distribution  of  Fig.  2  with the experimental conditions listed above. The Ramsey  spectra are normalised to the light intensity detected at the  end of the vapour cell in the absence of any microwave inter-rogation (i.e. Pm = 0). In the low microwave detuning region,  we obtain a good agreement between the Ramsey spectrum  measured using our POP Rb atomic clock and the computed  one.

4.2. Central fringe contrast

The variation of the contrast of the central Ramsey fringe in  Fig. 4 as a function of the microwave power corresponds to  the population oscillations in the ground state. It is equivalent  to the Rabi oscillations where the ground state population  varies  with  the  combined  microwave  pulse  area  2q.  Experi-mentally, we detect the change in the transmitted light at zero  microwave  frequency  detuning  as  a  function  of  the  micro-wave power. The contrast of the central fringe is defined as  the relative change in the optical absorption [5]: –10 –5 0 5 x

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mm –5 0 5 y

/

mm 0.75 0.80 0.85 0.90 0.95 1.00 10 x

/

mm 0 –10 0 y

/

mm 0 10 20 z

/

mm 10 0.2 0.4 0.6 0.8 1.0 N o rm al is ed H z N o rm al is ed H z a b

Figure 2. (a)  Simulated  microwave  magnetic  field  distribution  inside 

the vapour cell performed at the Laboratory of Electromagnetics and  Acoustics (LEMA-EPFL) and (b) transverse distribution of the mag-netic field at z = 9 mm. 1.0 0.9 0.8 0.7 0.6 –4000 –2000 0 2000 Wm

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Hz I(q = p/2)/I(q = 0) Figure 3. Simulated (solid curve) and measured (dashed curve) Ramsey  spectra. 0.5 0.4 0.3 0.2 0.1 0 btm/p 2.5 2.0 1.5 1.0 0.5 0 R(Pm)

Figure 4. Rabi  oscillations  simulated  for  (solid  curve)  homogeneous 

and  (dashed  curve)  inhomogeneous  microwave  field  and  (points)  measured Rabi oscillations (Ramsey spectrum central fringe contrast)  at Wm

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I I ( , ) ( , ) R 1 P 0 0 0 m m m W W = -= = .  (6)

The  quantity  R  obtained  numerically  as  well  as  experi-mentally is shown in Fig. 4. The results are consistent with the  Rabi oscillations measured using our POP Rb atomic clock  and with previously reported observations [5]. 4.3. Central fringe FWHM Figure 5 presents the FWHM of the central Ramsey fringe as  a function of btm. The central Ramsey fringe is obtained via  measurement  and  simulation  in  the  cases  of  homogeneous  and inhomogeneous microwave field amplitude distributions.  Let wH be the half width at half maximum (HWHM) of the  central fringe (wF = 2wH). Figure 5 presents the values of wF  determined from the wH solution of the equation: TRamsey wH + 2f0(b, wH) = p/2,  (7) where 

f0(b, wH) = arctan sincos( ( ) )

b t t 1 H H m m 2 w2 w xx + -e o.  (8)

A  good  agreement  between  the  inhomogeneous  micro- wave magnetic amplitude distribution case and the measure-ment  is  obtained.  Moreover,  we  obtain  a  good  agreewave magnetic amplitude distribution case and the measure-ment  between  the  homogeneous  microwave  magnetic  amplitude  case and wH solution of equation (7).

4.4. Central fringe frequency shift

Figure 6a presents the measured microwave-power sensitivity  of our DR POP clock. The frequency of the central fringe of  the Ramsey spectra simulated as a function of btm is shown  in Fig. 6b. The numerical calculation was performed taking  into account not only the microwave magnetic amplitude dis-tribution  of  Fig.  2  but  also  a  ground-state  frequency  shift  Df(r, t) dis tribution among the vapour cell. Two cases are con-sidered: homogeneous frequency shift distribution [Df(r, t) =  1  Hz]  and  inhomogeneous  frequency  shift  distribution.  In  order to reproduce the experimental data, at each point of the  mesh, we assumed the following empirical frequency shift dis-tribution that mimics a residual coherence at the end of the  optical pump pulse [12]: Df(r, t) = Cexp ( , )r t T sin ( , )rt T 1 1 op p op p 2 0 2 0 2 0 g d d d G G - + + + e e o o e o,  (9)

where  C  is  an  empirical  constant;  Gop(r, t)  is  the  optical  pumping rate; and d0 = 2D0 /G. The analysis of the physical  origins of this inhomogeneous shift will constitute the subject  of  a  separate  study.  Two  of  the  main  candidate  effects  are  however already identified: the AC Stark shift and the residual  coherence after optical pumping pulse.

5. Analysis and discussion

In  the  case  of  a  homogeneous  microwave  magnetic  field  amplitude  distribution,  all  the  atoms  in  the  vapour  cell  undergo the same microwave pulse. All the groups of atoms  produce the same Ramsey spectrum and are identical to the  output Ramsey spectrum. Its contrast is maximal for the (p/2  + np) pulse and is zero for (p + np) pulse. For a p pulse, no  fringes are observed and the FWHM cannot be defined, which  explains the discontinuity of the wF(btm) dependence at btm =  p in Fig. 5. For an inhomogeneous microwave magnetic field ampli-tude distribution, different groups of atoms in the vapour cell  undergo slightly different microwave pulses. It results that the  output Ramsey spectrum is an average of each Ramsey spec-trum  generated  inside  the  cell.  The  consequence  is  that  a  residual central fringe at btm = (p + np) is in this case present.  Thus a non-zero contrast (Fig. 4) and the wF (Fig. 5) can be  determined for btm = (p + np).

The  microwave-power  sensitivity  of  the  CFCF  is  repro-duced  as  consequence  of  two  inhomogeneities:  rubidium  ground-state resonance frequency shift distribution and micro-wF

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Hz 180 160 140 120 100 btm/p 2.5 2.0 1.5 1.0 0.5 0 Calculation Solution of Eqn (7) 1/(2TRamsey) Figure 5. Simulated FWHM of the Ramsey spectrum central fringe for 

( )  homogeneous  and  ( )  inhomogeneous  microwave  field  distribu-tions, and ( ) results of experimental measurements. 1.8 1.4 1.0 0.6 0.2 C lo ck f re q u en cy s h if t

/

H

z Laser frequency tuned on

|2S 1/2, F = 1ñ ® |2S1/2, F' = 0/F' = 1ñ |2S 1/2, F = 2ñ ® |2S1/2, F' = 3ñ 1.4 1.0 0.6 0.2 C en tr al f ri n ge fr eq u en cy s h if t

/

H z btm/p 0.8 0.6 0.4 0.2 0

Rb ground state frequency shift distribution homogeneous inhomogeneous b btm/p 0.8 0.6 0.4 0.2 0 a

Figure 6. (a)  Measured  microwave  power  sensitivity  of  the  clock 

fre-quency  and  (b)  simulated  microwave  power  sensitivity  of  the  central  fringe frequency. Frequency shifts are presented with respect to the fre-quency of 6.8346868658 GHz.

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wave  magnetic  field  amplitude  distribution.  The  output  Ramsey spectrum is an average of the Ramsey spectra gener-ated from each group of atoms in the vapour cell. Each group  of atoms has a contribution that depends on the microwave  pulses that they undergo. However, for a homogeneous reso- nance frequency shift distribution each group of atoms con-tributes with a different weight but with the same frequency  shift  (e.g.  no  shift  is  induced  by  the  microwave  coupling),  which explains the absence of microwave-power sensitivity of  the CFCF. In the case of an inhomogeneous resonance-fre-quency  shift  distribution,  the  inhomogeneous  microwave  field weights these various local shifts. When changing the  microwave power (q = btm µ  P tm m) the weight distribution  changes which gives rise to the microwave-power sensitivity  of the CFCF in Fig. 6.

Finally,  the  experimental  data  of  Fig.  6a  shows  that  an  operation point exists to reduce the microwave-power sensi-tivity coefficient in our POP DR clock. This occurs when the  laser frequency is tuned on the | 2S

1/2, F = 2 ñ ® | 2P3/2, F' = 3 ñ  transition  and  for  a  microwave  pulse  with  btm  =  0.57p.  In  this  condition,  we  measured  a  microwave-power  sensitivity  coefficient at the level of 4.5 ´ 10–14 mW–1 which is two orders  of  magnitude  lower  than  the  previously  reported  coefficient  [17].  Operating  our  DR  POP  clock  in  these  conditions,  we  have  reported  a  long-term  relative  frequency  stability  of  1 ´ 10–14 [18].

In conclusion, we have analysed the impact of the micro-wave  magnetic  field  amplitude  inhomogeneity  on  Ramsey  spectroscopy.  Based  on  a  theoretical  model  describing  the  Ramsey  spectroscopy,  we  demonstrated  the  impact  of  the  microwave field amplitude inhomogeneity and the resonance-frequency distribution on the Ramsey spectrum, in particular  on the contrast, the FHWM, and the frequency detuning of  the central fringe. We obtained excellent agreement between  the numerical simulation and the measurement in each case.  Especially, we demonstrated that the microwave-power sensi-tivity of our POP DR atomic clock can be reproduced from  the  presence  of  two  inhomo geneities:  microwave-power  inhomogeneity and atomic resonance frequency inhomogene-ity. Further studies are necessary in order to study and ideally  suppress the latter.

Acknowledgements. This  work  was  supported  by  the  Swiss  National Science Foundation (SNSF Grant No. 156621). The  authors thank M. Dürrenberger and P. Scherler (both LTF,  University of Neuchâtel, Switzerland) for technical support.  We also thank A. Skrivervik and A.E. Ivanov (EPFL-MAG,  Switzerland) for fruitful collaborations on microwave cavity  developments and simulations. 

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Figure

Figure 1.  (a)  Double-resonance  interaction  scheme,  (b)  POP  timing  scheme,  and  (c)  three-level  approximation  of  the  87 Rb  D 2   line.  Here,  H z  is magnetic field strength of the microwave signal;  w L  and  w m  are the  optical and micro
Figure 3 presents the calculated light intensity at the end of  the  vapour  cell  I(q  =  p/2)  as  a  function  of  the  microwave  frequency detuning W m  and the measured Ramsey spectrum. 
Figure 6a presents the measured microwave-power sensitivity  of our DR POP clock. The frequency of the central fringe of  the Ramsey spectra simulated as a function of bt m  is shown  in Fig. 6b. The numerical calculation was performed taking   into accoun

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